CN106029606A - 陶瓷材料和包含所述陶瓷材料的电容器 - Google Patents

陶瓷材料和包含所述陶瓷材料的电容器 Download PDF

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CN106029606A
CN106029606A CN201580009101.8A CN201580009101A CN106029606A CN 106029606 A CN106029606 A CN 106029606A CN 201580009101 A CN201580009101 A CN 201580009101A CN 106029606 A CN106029606 A CN 106029606A
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ceramic material
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京特·恩格尔
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Abstract

本发明涉及一种用于电容器的陶瓷材料。为了实现将所述材料装配到具有反铁电性质的多层电容器时减少的自发热和高的介电常数，具有式[Pb(1‑r)(BaxSryCaz)r](1‑1.5a‑1.5b‑0.5c)(XaYb)Ac(Zr1‑dTid)O3的陶瓷材料被提出，其中X和Y都代表稀土金属，所述稀土金属选自由La，Nd，Y，Eu，Gd，Tb，Dy，Ho，Er和/或Yb组成的组；其中A代表一价离子；x+y+z＝1；x和/或y和/或z>0；0<r<0.3；0<d<1；0<a<0.2；0<b<0.2；0<c<0.2。

Description

陶瓷材料和包含所述陶瓷材料的电容器
本发明涉及一种陶瓷材料。
此外，本发明涉及这种类型材料的用途。
最后，本发明还包括电容器，尤其是多层电容器。
电容器被用于电气工程的很多领域，例如用于电机驱动装置的AC/DC变换器，以及例如，用于在DC/DC电路中提高电压、降低电压和/或稳定电压。在这种类型的应用中，往往提供具有二极管的半导体开关(被称为“逆变器电路”)和额外的电路，其中电容器被放置在这些电路之间，这种电容器也被称为中间电路电容器。为了提高电压参数和电流参数，串联和并联多个电容器也由此成为可能。
在提到的中间电路电容器的情况中，操作多变电流和电压时，在急速发生的并且数量上显著的改变期间，放置在额外电路之间的电容器具有保持中间电路电压稳定的任务。通常由此而产生的问题是，因为电容器所处的环境，电容器设计的可能性受到了半导体以及由基板和必需的导线引发的要求的限制。由此而论，电容器的期望理想参数被具有半导体元件的电路的低于理想情况的次级属性伴随和/或影响就尤其成问题，这些属性能够显著影响设计的限制。这些限制性的次级属性也被称为“寄生”次级属性。
对于半导体，存在不同组件的若干种类，每一种都具有特定的优点和缺点。基于硅的半导体开关是公知的，例如，绝缘栅双极型晶体管(IGBT)或者金属氧化物半导体场效应晶体管(MOSFET)，和具有除硅外其他基础材质的相应组件，尤其例如砷化镓(GaAs)、氮化镓(GaN)或碳化硅(SiC)。所有之前提到的组件，尽管具有特定的优点，但是，都具有提到的寄生属性。这些属性对各种期望的功能几乎都存在。例如，存在这样的结果，期望的高电流通过已知的式子U＝-L dl/dt快速转换，即对高电流(大dl)快速的转换操作(小dt)，甚至是低感应系数L和高(过)电压，所述感应系数由自感和线路电感构成，所述电压会造成半导体自损坏。据此，如果要求这种类型的问题永久性地得到解决的话，适当的设计措施和反措施是必需的。为了解决这个问题，中间电路电容器典型地是过大的，一方面是为了切断过电压，另一方面是为了补偿由于寄生串联阻抗导致的半导体的栅电容减少的充电/放电率。因此，应用环境决定了电容器的设计。
另一个寄生属性是泄露电流，其几乎总是导致巨大的温度升高，而温度升高必须被限制在一定的允许量级内。虽然就这一点而言准确地说，半导体在更高的温度下非常坚固并且尤其高效，但是，过分的温度和/或重复的材料-压力温度改变最终会导致这些元件中的材料损坏，或者至少限制连接到半导体或者位于半导体邻近位置的材料的使用寿命，例如基板或者连接器件，尤其是电容器也是如此。
关于热稳定性，电容器具有窄的限制，尤其是在高电流和高电压情况下使用时。对于所有电容器技术，由于随着温度不断升高，泄露电流升高并且阻断电压降低，这点也必须在设计时考虑到。因为电路中的半导体产生热量，以及由于电容器自身对温度升高的贡献，除了在任何情况下都要使电容器过大之外，将电容器安置在距离半导体一定的距离的位置，以能够有效冷却，从而使温度处于预设的范围内，在先前就已经是有必要的了。然而，由于这样的间隔，要求的更长的电连接总是具有相应的电感，所述电感在上述式子方面是反生产的，并且使电容器的额外的过大成为必需。
在现有技术中，各种各样的电容器技术已经被大家所知道，尤其是陶瓷多层电容器，铝电解质电容器和金属薄膜电容器。具体地，电容、电压、脉动电流、等效串联电阻、损耗系数、频率响应、电容稳定性和降额电压被用作用于特殊使用目的的评估参数，温度特性，可靠性，能量密度和成本也是。鉴于这些评估参数和标准，铝电解质电容器和金属薄膜电容器主要在能量范围起于大约1kW的情况下使用，而陶瓷电容器在比所述能量范围更低的能量范围下使用。
组件向小型化方向发展的一般趋势也适用于电可移动设备，并且因此，对于一些组件，如之前提到的用于电机驱动装置的AC/DC变换器也是如此。对于与逆变器相关的电子组件，存在被设计的显著更小且更有效的需求。关于电容器，如果随着电压的升高直到逆变器要求的高电压为止将被使用的X7R电容器的电容不会降低，那么，陶瓷多层电容器的性能优于铝电解质电容器或者金属薄膜电容器(M.ECPE汽车电力电子路标，ECPE-HOPE汽车电力电子研讨会，2008年10月7-8日)。例如，在典型的电压大约400V左右，电容因此降低到例如额定值的25％；另外，能量存储仅仅通过电场力产生，几乎没有任何偏振组件的增加。然而，已知一些材料，电容最初增加，达到最大值，之后才再次衰减(US 7781358；(C.K.Campell等，组件和包装技术的IEEE会报，2002年，第25卷第2期，211页))。对于操作电压，能量存储也通过偏振能达到一个很高的程度。在应用条件下，可获得的高容量密度由此证明是显著的优点，其与常规陶瓷电容器相反。然而，由于一个显著的缺点，相当贵重的金属钯或者银/钯合金被用作这些材料的内部电极。这在单个应用中尚可接受，例如医药设备，但是作为广泛的经济应用不可取。
替代钯或者银/钯合金，通过调整电容器中陶瓷材料的组成，使用铜作为内在电极最近也成为可能(WO 2013/152887 A1)。这种类型的电容器呈现出卓越的高频率性能。另外，铜是划算的。具有铜作为内在电极以及基于锆钛酸铅(PZT)的陶瓷基组件的相应多层电容器也已经在要求高性能的电子设备中使用。然而，自热的问题仍然存在。
基于所呈现的现有技术，本发明的目标是详细说明具有高的介电系数并适用于生产具有低自热的电容器，尤其是多层电容器，的陶瓷材料，因此，所述陶瓷材料可以被安置紧邻半导体。
此外，本发明的目标是阐明这种类型材料的用途。
最后，本发明的目标是详细说明在使用过程中具有低自热高性能的电容器。
第一个目标是通过具有下式的陶瓷材料被达成：
[Pb(1-r)(BaxSryCaz)r](1-1.5a-1.5b-0.5c)(XaYb)Ac(Zr1-dTid)O3
其中
X和Y分别是稀土金属，所述稀土金属选自包括镧(La)，钕(Nd)，钇(Y)，铕(Eu)，钆(Gd)，铽(Tb)，镝(Dy)，钬(Ho)，铒(Er)和/或镱(Yb)的组；
A代表一价离子；
x+y+z＝1；
x和/或y和/或z>0；
0<r≤0.3；
0≤d≤1；
0≤a≤0.2；
0≤b≤0.2；
0≤c≤0.2。
本发明概念上的范围包括这样的想法，电容器中的陶瓷材料使用过程中的自热可以被减少，因此充放电操作被促进。这个想法出发点是，在反铁电材料中，介电位移依赖于电容器材料的结构态，宏观偏振由离子单位微观取向进行，反之亦然。在这种情况下，充放电操作可以被看做是偏振波，偏振波的载体是偏振晶格的晶格振动。这些晶格振动是结构依赖的并且具有特定的频率和能量密度。根据现有技术，反铁电材料的基础结构是由钛酸盐八面体在顶点连接形成的ABO3型钙钛矿结构，其中能量较低的晶格振动构成第一近似所述八面体耦合的倾斜/转动的振动。取决于陶瓷的形态，八面体的倾斜角决定了各种相态(反铁电相，铁电相或顺电相)。介电常数和损失角的量级分别对应于振幅和振动衰减。
根据所考虑的内容，准确地说，这些集合的晶格振动在结构水平上应该更加容易可激发，这是理论考虑内容的第一个方面。
考虑的第二个方面是，在多层电容器里期望使用划算的铜内电极。对于这些电容器，必须要额外克服的问题是仅允许低的烧结温度。然而，为了借助于烧结助剂促进烧结而不得不产生的缺陷结构在组成方面只能在很窄的限制范围内进行调整。为此，根据现有技术，单价掺杂离子被使用，所述离子大概被引入至这样的程度，以至于对于反铁电相关键的离子针对价态被补偿。作为发明的一部分，现已经发现，晶格动力学的有目标控制开启了在保持典型的烧结助剂的同时降低自热的可能性。本发明基于这样的概念，当倾斜/转动的振动在静止位置周围具有能量平的发展时，自热将是最低的。应用于钙钛矿结构，这意味着结构相转化可以被近似。根据本发明，这通过将铅(Pb)部分替换为钡(Ba)来实现。在进一步的实施方案中，晶格间隙可以被锶(Sr)和钙(Ca)补偿。然而，因为结构相转化会阻碍反铁电相的形成，由于这个原因，相转化仅仅只能被近似，Ba，Sr和Ca的含量必须被调整以使0<r≤0.3。
先前提到的考虑内容的具体实施表明，通过使用Ba，Sr和/或Ca来部分取代Pb，反铁电陶瓷材料的结构可以被调整以至于：一方面，在电容器中使用期间自热显著减少；另一方面，优选的铜内电极可以在多层电容器中应用。也可以取代Ba的锡(Sn)不被采用，由于即使使用Sn可能会降低自热，但是，在这种情况下，伴随使用铜内电极时的同样的期望的烧结能力不能得到保证。
根据本发明，为了对晶格或者材料形成产生有利的影响，0.01≤r≤0.2是优选的。
陶瓷材料以以下值实施是尤其优选的：
0.01≤x<1；
0≤y≤0.99；
0≤z≤0.2。
如果Ba是必需采用的，那么由于优化的结构导致所述材料在电容器中使用期间有低的自热。这被针对于晶格间隙的优化的Sr和Ca的可能存在进一步加强。
如果只有Ba被采用，所述材料呈现：
y和z＝0；
0.1≤r≤0.2。
如果采用0<y≤0.99的实施方案，其中Ba含量大于Sr含量，多层电容器中的损失角以及由此的自热可以被尤其有效的最小化。
为了进一步强化，Ba与Sr和/或Ca同时存在可以被采用，
其中
0.01≤x<1；
0<y≤0.99；
0<z≤0.2；
因此，在所述材料在多层电容器中使用期间，损失角和由此的自热可以被减少直至80％。至于锆(Zr)和钛(Ti)的含量，优选的具体范围是0.01≤d≤0.70，尤其是0.03≤d≤0.52。
一价离子A本身并不是决定性的，但是优选地选自包括钠(Na)、钾(K)、锂(Li)和/或银(Ag)的组，其中，Na被证明在降低烧结温度方面尤其有用，从而对铜内电极的烧结能力尤其有用。一价离子A，尤其是Na，可以以3％到7％，或者0.03≤c≤0.07，尤其是0.04≤c≤0.06的低含量存在。相应的含量已经足够来降低烧结温度到最大1050℃，其代表了使用铜内电极时的最大烧结温度。在一价离子中，Na,K和Li比Ag更优选，其中以上所有的一价离子中，Na被证明尤其合适。
作为稀土金属，优选地，镧(La)单独使用或者与钕(Nd)组合使用。在通常可以用ABO3表示的钙钛矿结构中，其中A和B分别代表A空间和B空间，稀土金属占据A空间代替Pb。由于La和ND是三价的，像之前提到的其他稀土金属，这是一个给体掺杂，所述给体掺杂被受体掺杂用一价离子A补偿。这种共掺杂对最高可能的介电系数是有利的。La尤其优选，其中，优势的含量是0.04≤a≤0.18，尤其是0.04≤a≤0.16，例如0.04≤a≤0.07可以被采用。在这种情况下，Nd可以被省略，所以b＝0。
根据依照本发明的陶瓷材料的上述阐明的优点，所述材料优选被使用在电容器中，尤其是多层电容器。
本发明将在下文中借助示例性的实施方案被更详细的解释。
以下描述的陶瓷材料可以使用传统的混合氧化过程获得，即将基于例如氧化物、醋酸盐、硝酸盐和/或碳酸盐的前驱体在1000℃到1150℃的温度范围内烧结。可替换地，溶胶-凝胶法也可以用来在初始阶段将金属醋酸盐和/或金属醇盐的溶液形成溶胶，所述溶胶通过干燥和后续煅烧的手段转化为最终的陶瓷材料。
下表1中列出的实施例依照混合氧化的方法被生产，其中制造的反铁电材料的通式如下：
[Pb(1-r)(BaxSryCaz)r](0.65)(La0.1Nd0.1)Na0.1(Zr0.6Ti0.4)O3
不同含量的Ba，Sr和/或Ca构成部分的起始材料，所述起始材料被烧结，并且以这种方式被引入到最终材料中。
表1：示例性的实施方案
实施例 r x(Ba) y(Sr) z(Ca) 丢失角减少[％]
1 0.2 1.0 0.0 0.0 70
2 0.15 0.66 0.34 0.0 80
3 0.15 0.66 0.27 0.07 80
如表1，通过Ba，Sr和/或Ca的掺合，丢失角可以被减少70％到80％，这导致材料在多层电容器中使用时自热相应减少。
如果Zr和Ti的含量被调整，还是可以获得相似的结果，例如，具有Ba，Sr和/或Ca替换的陶瓷材料的通式如下：
[Pb(1-r)(BaxSryCaz)r](0.65)(La0.1Nd0.1)Na0.1(Zr0.9Ti0.1)O3
由于自热被极大减少，所以，具有根据本发明的陶瓷材料和安置于其间的铜内电极的多层电容器尤其适用于空间-节约电路。以这种方式，例如将多层电容器安置在多个半导体二极管之间成为可能，从而制造了具有最小的可能损失的空间优化结构，并使电磁辐射最小化。

Claims (15)

1.一种具有下式的陶瓷材料：
[Pb(1-r)(BaxSryCaz)r](1-1.5a-1.5b-0.5c)(XaYb)Ac(Zr1-dTid)O3
其中
X和Y分别是稀土金属，所述稀土金属选自包括La，Nd，Y，Eu，Gd，Tb，Dy，Ho，Er和/或Yb的组；
A代表一价离子；
x+y+z＝1；
x和/或y和/或z>0；
0<r≤0.3；
0≤d≤1；
0≤a≤0.2；
0≤b≤0.2；
0≤c≤0.2。
2.如权利要求1所述的陶瓷材料，其中
0.01≤r≤0.2。
3.如权利要求1或2所述的陶瓷材料，其中
0.01≤x<1；
0≤y≤0.99；
0≤z≤0.2。
4.如权利要求3所述的陶瓷材料，其中
y和z＝0；
0.1≤r≤0.2。
5.如权利要求3所述的陶瓷材料，其中
0<y≤0.99；
Ba含量大于所述Sr含量。
6.如权利要求3所述的陶瓷材料，其中
0.01≤x<1；
0<y≤0.99；
0<z≤0.2；
Ba含量大于所述Sr含量，Sr含量大于所述Ca含量。
7.如权利要求1到6之任一项所述的陶瓷材料，其中
0.010≤d≤0.70，特别地0.03≤d≤0.52。
8.如权利要求1到7之任一项所述的陶瓷材料，其中A选自包括Na，K，Li和/或Ag的组。
9.如权利要求1到8之任一项所述的陶瓷材料，其中X代表La，Y代表Nd。
10.如权利要求1到9之任一项所述的陶瓷材料，其中所述的材料是反铁电的。
11.一种如权利要求1到10之任一项所述的陶瓷材料用于电容器，特别是多层电容器的用途。
12.一种包括如权利要求1到10之任一项所述的陶瓷材料的电容器。
13.一种包括至少一层如权利要求1到10之任一项所述的材料的多层电容器。
14.如权利要求11所述的多层电容器，其中内部电极是由铜形成的。
15.一种包括如权利要求13或者14所述的多层电容器的用于电机驱动装置的逆变器。
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